Smith will play the notorious serial killer in the film "Charlie Says", according to The Hollywood Reporter.
The film will revolve around three young women, who were sentenced to death for their role in the Manson murders but it was later converted to a life sentence.
The story will be told through a graduate student, who is tasked with re-educating the women as they come to terms with their horrific crimes under the influence of Manson.
Suki Waterhouse, Merrit Wever, Carla Gugino, Hannah Murray, Kaylie Carter and Marianne Rendon have also joined the cast the drama.
Harron is not new to dark stories as her creation of Patrick Bateman in "American Psycho" is now a part of movie cult.
Bateman, memorably played by Christian Bale, is a wealthy young investment banker who turns into a serial killer by night.
In the late 1960s, Manson formed a cult in California, which came to be known as the Manson Family. The cult members committed a series of nine murders.
They gained national notoriety after the murder of director Roman Polanski's actor-wife Sharon Tate and four others in her home in 1969.
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